The power of magnetic resonance (MR) techniques, including nuclear magnetic resonance (NMR) and electron spin resonance (ESR) has been significantly increased in recent years by the inclusion of added dimensions in the Fourier domain, expanding the ability to determine molecule structure, dynamics, and kinetics. MR techniques have also been advanced by the development of multi-dimensional diffusion/relaxation pulse sequences through the use of robust and accurate two-dimensional (2D) inverse Laplace transform (ILT) algorithms and data analysis methods. However, the amount of 2D MR relaxation data and the time required to acquire this data makes 2D relaxometry infeasible and/or impractical. This limitation is particularly severe if one attempts to combine MR relaxometry methods with magnetic resonance imaging (MRI).